title: Structural origin of dynamic heterogeneity in three-dimensional colloidal glass formers and its link to crystal nucleation.
abstract: The physical understanding of glass transition remains a major challenge of physics and materials science. Among various glass-forming liquids, a colloidal liquid interacting with hard-core repulsion is now regarded as one of the most ideal model systems. Here we study the structure and dynamics of three-dimensional polydisperse colloidal liquids by Brownian dynamics simulations. We reveal that medium-range crystalline bond orientational order of the hexagonal close packed structure grows in size and lifetime with increasing packing fraction. We show that dynamic heterogeneity may be a direct consequence of this transient structural ordering, which suggests its origin is thermodynamic rather than kinetic. We also reveal that nucleation of crystals preferentially occurs in regions of high medium-range order, reflecting the low crystal-liquid interfacial energy there. These findings may shed new light not only on the fundamental nature of the glass transition, but also the mechanism of crystal nucleation.
authors.affiliation: Institute of Industrial Science, University of Tokyo, 4-6-1 Komaba, Meguro-ku, Tokyo 153-8505, Japan.
authors.forename: Takeshi
authors.initials: T
authors.lastname: Kawasaki
authors.forename: Hajime
authors.initials: H
authors.lastname: Tanaka
mesh_terms: D003102:Colloids / Q000737:chemistry*; D003460:Crystallization; D005898:Glass / Q000737:chemistry*; D007700:Kinetics; D008958:Models, Molecular; D008968:Molecular Conformation; D010825:Physics / Q000379:methods; D013816:Thermodynamics
chemical_list: D003102:Colloids